Asphalt emulsion

ABSTRACT

An asphalt emulsion comprising water, asphalt, (A) an emulsifier selected from the group consisting of specific aliphatic amines, aminated lignins, imidazolines having a hydrocarbon group having 7 or more carbon atoms, and amidobetaines having a hydrocarbon group having 7 or more carbon atoms, (B) a polyphenolic compound, and (C) at least one member selected from the group consisting of anionic polumeric dispersants, hydroxycarboxylic acids and/or (D) at least one member selected from the group consisting of saccharides, sugar alcohols and polyhydric alcohols, which is excellent in storage stanility, mixability with aggregate and low foaming properties of the emulsion itself, in adherence of the products of breaking thereof to aggregate, and in stripping resistance of the construction executed by the use of the emulsion.

BACKGROUND ART

1. Technical Field

The present invention relates to an additive composition for asphaltemulsion, a composition for asphalt emulsion and a composition foremulsification which are used for the preparation of an asphaltemulsion; an oil-in-water asphalt emulsion; a paving compositioncomprising aggregate and an oil-in-water asphalt emulsion; and a processfor the preparation of the above composition for emulsification. Theasphalt emulsion according to the present invention is excellent instability as emulsion and mixability with aggregate, and is easy tocontrol the decomposition time thereof, and the products (mainlyasphalt) of breaking of the emulsion are excellent in adherence toaggregate. Further, the constructions executed by the use of theemulsion are excellent in stripping resistance. Other asphalt emulsionsaccording to the present invention are used by mixing it with aggregatein plant or place in the use of open grade mixtures, dense grademixtures, slurry seals, sand mixtures, reclaimed mixtures and so on, areexcellent in stability as emulsion, mixability with aggregate andmixability with cement, and is easy to control the decomposition timethereof, and the products (mainly asphalt) of breaking of the emulsionsare excellent in adherence to crushed stone. Further, the constructions,such as pavement, executed by the use of the emulsions are excellent instrength, endurance and stripping resistance.

2. Description of the Related Art

Bituminous materials obtained from petroleum, e.g., asphalt, tar andpitch, have widely been used from old as a paving material, a waterproofmaterial and an adhesive and in the construction of railroads. However,bituminous materials are very poor in workability when used as such,owing to their extremely high adhesivenesses. Therefore, bituminousmaterials are used after their flowabilities are enhanced by a meanssuch as heating (i.e., heat melting process), treatment to be in theform of emulsion by using a proper emulsifying agent and water, anddissolution in a suitable solvent, for securing a desirable workability

Among such emulsions of bituminous materials, aqueous emulsions ofasphalt are generally called "asphalt emulsions". Such the asphaltemulsions are roughly classified into fast-decomposing emulsions (i.e.,emulsions for application) which are directly applied to the objectsurface, and slow-decomposing ones (i.e., emulsions for blending) whichare blended with aggregate. Although the surfactant to be used in thepreparation of an asphalt emulsion is suitably selected from amonganionic surfactants, cationic surfactants, nonionic surfactants andamphoteric surfactants, the kind thereof is generally determineddepending upon the process of execution thereof.

Among the above asphalt emulsions, one for blending is mixed withaggregate, a filler and other components. The asphalt composition thusprepared is used for the construction of paving of a road. The so-calledemulsion breaking is caused by the evaporation and elimination ofaqueous components in the composition, after the execution of a road byusing an asphalt composition. Thus, the asphalt is hardened to completethe construction of paving of a road.

Further, the kind of paving of a road to be formed and the propertiesand performance thereof vary depending upon the kind of aggregate to beused together with such the emulsion for blending. For example, anasphalt composition (an open grade mixture) comprising an emulsion forblending and an open grade aggregate is used in the execution of upperand lower subbases, or in the execution of surface drainage course.While an asphalt composition (a dense grade mixture) comprising anemulsion for blending and a dense grade aggregates is used in theexecution of upper subbase or surface course. Further, a compositionprepared by mixing an emulsion for blending with a fine aggregate orfiller is used as slurry seal for the purpose of restoring adeteriorated area of pavement, and a composition (a sand mixture)prepared by mixing it with sand is used for forming a simple surfacecourse. It is also conducted to mix an emulsion for blending withcrushed paving (a reclaimed mixture), for the re-use of deteriorated andexisting paving. Meanwhile, the mixing processes for preparing such theasphalt compositions include two processes, i.e., in-plant mixing andin-place mixing, and they are used properly and suitably depending uponthe conditions.

In the execution of a road by using an asphalt emulsion for blending,the asphalt which is re-generated by breaking the asphalt emulsionadheres to aggregate to act as a binder among the aggregate, by whichthe strength and endurance of paving of a road are exhibited. Meanwhile,as described above, an asphalt emulsion for blending contains asurfactant. An emulsion containing, among surfactants, an anionicsurfactant or a nonionic surfactant has a significant disadvantage inthat the products, mainly asphalt, of breaking of the emulsion are poorin adherence to aggregate, though the emulsion has such an advantagethat it exhibits good mixability with aggregate. On the other hand, acationic surfactant accelerates the adhesion of asphalt particles toaggregate by the electric attractive force thereof. However, paving of aroad executed by the use of an asphalt emulsion containing a cationicsurfactant is also poor in strength and endurance. Thus, it has become acommon opinion that every paving of a road executed by the use of anasphalt emulsion is poor in strength and endurance. Although thestrength and endurance of paving of a road executed by the use of anasphalt emulsion are, as described above, exhibited by the adhesion ofasphalt to aggregate, the strength and endurance of paving of a roadexhibited by the use of a current asphalt emulsion are insufficient, andmeasures for improvement by which higher strength and endurance can berealized are desired.

Additionally, it is required for an asphalt emulsion for blending tohave such performances that the stability of the emulsion is excellentwhen a forced mechanical agitation is conducted, that it does not causeseparation (i.e., an emulsion breaking is not occurred) during executionsuch as transportation, spreading and rolling, that it is separated(i.e., the emulsion is broken) at a somewhat high speed after paving,that the products of breaking of the emulsion is excellent in adherenceto aggregate, and that these various properties are not affected by thekind of aggregate, atmospheric temperature at execution and so on. Asmeasures for satisfying these requirements, there have been proposed theuse of a large amount of an emulsifier (surfactant), the use of manykinds of emulsifiers, and the addition of a water-soluble organicpolymer, e.g., polyvinyl alcohol, gelatin, methylcellulose,polyacrylamide or guar gum, to an asphalt emulsion as a protectivecolloid. An asphalt emulsion is stabilized by carrying out suchmeasures. However, by carrying out these measures, such the effect thatthe adherence of the products, mainly comprising asphalt, of breaking ofthe emulsion to aggregate is essentially improved by the improvement ofthe properties of interface between aggregate and asphalt, is attained.

Various methods for improving the various properties of an asphaltemulsion have been proposed in addition to the those described above.

For example, there have been proposed the use of an aminated lignin, analkylimidazoline compound and a nonionic emulsifier (see U.S. Pat. No.3,871,893), that of a fatty acid salt of an alkylimidazoline compound(see U.S. Pat. No. 3,979,323), and that of a specific nonionicemulsifier (see Japanese Patent Publication-A No. Hei 7-118538) forimproving the mixability of an asphalt emulsion with aggregate and theadherence properties of the products of breaking of the emulsion toaggregate. By these techniques, the mixability of an asphalt emulsionwith aggregate is improved. Even when such an asphalt emulsion is used,however, the adherence of asphalt to aggregate and the strippingresistance of paving executed are insufficient owing to the interventionof water. Thus, the paving does not exhibit sufficient strength andendurance, only by measures of selecting the surfactant. Further,Japanese Patent Publication-A No. Sho 57-42763 and U.S. Pat. No.3,867,162 disclose the use of a saturated fatty acid and that of talloil fatty acid, respectively. However, an asphalt emulsion containingsuch an organic acid cannot be used in the case wherein cement orferrous slag, which is basic, is used. Additionally, it cannot beexpected under the current circumstances wherein lowering in the qualityof road asphalt or aggregate is apprehended and, on the other hand, theuse of reclaimed materials also spreads that excellent mixability of theemulsion with aggregate and firm adhesion of the components, such asasphalt, in the products of breaking of the emulsion to aggregate areexhibited by the use of an asphalt emulsion containing such an organicacid.

It is described in Japanese Patent Publication-A No. Sho 63-17960 thatby allowing an asphalt emulsion to contain tannic acid or a tannincompound, the mixability of the emulsion with aggregate, the adherenceof, e.g., asphalt to aggregate, and the stripping resistance of thepaving which has been executed with the use of the emulsion areimproved, and the decomposition time of the emulsion is prolonged. In anasphalt emulsion containing tallow-alkyl propylene-diamine,polyoxyethylene tallow-alkyl propylenediamine orstearyltrimethylammonium chloride which is a cationic surfactant, whichis described in the above Publication, the delay of the decompositiontime thereof is certainly attained by the addition of tannic acid.However, even in such the case, the decomposition time is still tooshort for the use of the asphalt emulsion as one for blending. Further,when tannic acid or a tannin compound is to be contained in an asphaltemulsion containing a nonionic surfactant such as polyoxyethylenenonylphneyl ether or an anionic surfactant such as sodium oleate, theadherence of the components such as asphalt in the products of breakingof the emulsion to aggregate is remarkably lowered, and thus thesufficient strength and endurance of a paving can not be obtained,though the mixability of the emulsion with aggregate is improved.

As described above, there has not been known an asphalt emulsion whichis one to be used for the preparation of a composition (for example, anopen-grade mixture, a dense grade mixture, a slurry seal, a sand mixtureor a reclaimed mixture) for paving a road comprising an asphalt emulsionfor blending and aggregate and which satisfies all of the propertiesincluding stability as emulsion, mixability with aggregate, easiness ofcontrolling the decomposition time, adherence of the products ofbreaking thereof to crushed stone, and stripping resistance, strengthand endurance of the paving executed by the use of the emulsion, thedevelopment thereof has been eagerly desired and the development thereofhas been highly expected.

DISCLOSURE OF THE INVENTION Summary of the Invention

The present inventors have extensively studied to solve the aboveproblems according to the asphalt emulsion. As a result of the studies,the present inventors have found that by adding a polyphenolic compoundwhich not only acts as a protective colloid for the asphalt particles inan asphalt emulsion but also exhibits adherent affinity for aggregate,and a dispersant for inorganic materials such as clay, powdered stoneand cement and/or a water-holding component to an aqueous emulsifiersolution which is used for the emulsification of asphalt, the synergismbetween them is exhibited, and the emulsion stability, mixability withaggregate and mixability with cement of the asphalt emulsion, theadherence of the products, such as asphalt, of breaking of the emulsionto aggregate, and the stripping resistance and strength of the pavingexecuted with the use of the emulsion are remarkably improved. Thepresent invention has been accomplished on the basis of this finding.

Thus, the first embodiment of the present invention relates to anadditive composition for asphalt emulsion which comprises (B) apolyphenolic compound, at least one member selected from the groupconsisting of (C) anionic polymeric dispersants, hydroxycarboxylic acidsand water-soluble salts of hydroxycarboxylic acids and (D) saccharides,sugar alcohols and polyhydric alcohols and, optionally, (A) anemulsifier.

Further, the second embodiment of the present invention relates to anasphalt emulsion comprising asphalt, water, (A) an emulsifier, (B) apolyphenolic compound and at least one member selected from the groupconsisting of (C) anionic polymeric dispersants, hydroxycarboxylic acidsand water-soluble salts of hydroxycarboxylic acids and (D) saccharides,sugar alcohols and polyhydric alcohols.

The asphalt emulsion of the second embodiment of the present inventionincludes an asphalt emulsion characterized by containing (A) anemulsifier, (B) a polyphenolic compound and one or more compoundselected from among (C) anionic polymeric dispersants, orhydroxycarboxylic acids or water-soluble salts thereof, and/or (D)saccharides, sugar alcohols and polyhydric alcohols, as essentialcomponents.

Furthermore, the third embodiment of the present invention relates to apaving composition which is used for, e.g., paving a road, comprisingaggregate and the asphalt emulsion of the second embodiment of thepresent invention.

The fourth embodiment of the present invention relates to use of theadditive composition for asphalt emulsion according to the firstembodiment for preparing an asphalt emulsion.

The fifth embodiment of the present invention relates to a compositionfor emulsification which comprises water, (A) an emulsifier, (B) apolyphenolic compound, and at least one member selected from the groupconsisting of (C) anionic polymeric dispersants, hydroxycarboxylic acidsand water-soluble salts of hydroxycarboxylic acids and (D) saccharides,sugar alcohols and polyhydric alcohols.

The composition for emulsification of the fifth embodiment of thepresent invention may further contain a monobasic acid.

The sixth embodiment of the present invention relates to a process forthe preparation of the composition for emulsification of the fifthembodiment of the present invention containing components (C) and (D),which comprises step 1 of adding a mixture of component (A) andcomponent (D) to an aqueous solution of component (B) to prepare anaqueous solution and step 2 of adding an aqueous solution of component(C) to the obtained solution.

The seventh embodiment of the present invention relates to a process forthe preparation of the composition for emulsification of the fifthembodiment of the present invention containing components (C) and (D)and a monobasic acid, which comprises step 1 of adding a monobasic acidto an aqueous solution of component (B) to prepare an aqueous acidicsolution, step 2 of adding a mixture of component (A) and component (D)to the aqueous acidic solution to prepare an aqueous solution, and step3 of adding an aqueous solution of component (C) to the obtained aqueoussolution.

The eighth embodiment of the present invention relates to a process foremulsifying asphalt in water, which comprises adding molten asphalt tothe composition for emulsification of the fifth embodiment of thepresent invention to prepare a mixture, and then emulsifying themixture.

The ninth embodiment of the present invention relates to use of thecomposition for emulsification of the fifth embodiment of the presentinvention for emulsifying asphalt.

Further, the present inventors have made extensive studies also on anasphalt emulsion which is applicable to the case where particularly highstrength and endurance are necessitated in a paving executed with theuse of the emulsion. As a result of the studies, the present inventorshave found that by adding (A) at least one surfactant selected from thegroup consisting of specific aliphatic amines, aminated lignins,imidazolines having a hydrocarbon group having 7 or more, preferably 8or more, carbon atoms, betaines having a hydrocarbon group having 7 ormore, preferably 8 or more, carbon atoms and amidobetaines having ahydrocarbon group having 7 or more, preferably 8 or more, carbon atoms,(B) a polyphenolic compound and, optionally, at least one memberselected from the group consisting of (C) anionic polymeric dispersants,hydroxycarboxylic acids and water-soluble salts of hydroxycarboxylicacids and (D) saccharides, sugar alcohols and polyhydric alcohols in thepreparation of an asphalt emulsion, the emulsion stability, mixabilitywith aggregate and mixability with cement of the asphalt emulsion, andthe easiness of controlling the decomposition time are improved, theadherence of the components, such as asphalt, in the products ofbreaking of the emulsion to crushed stone is also improved, and thestripping resistance, strength and endurance of the paving executed withthe use of the emulsion is enhanced. The present invention has beenaccomplished on the basis of this finding.

A tenth embodiment of the present invention relates to a composition forasphalt emulsion which comprises (A-1) at least one member selected fromthe group consisting of aliphatic amines represented by the followingformula (1), aminated lignins, imidazolines having a hydrocarbon grouphaving 7 or more, preferably 8 or more, carbon atoms, betaines having ahydrocarbon group having 7 or more, preferably 8 or more, carbon atomsand amidobetaines having a hydrocarbon group having 7 or more,preferably 8 or more, carbon atoms, and (B) a polyphenolic compound:##STR1## wherein R¹ is a hydrocarbon group or acyl group having 8 to 22carbon atoms; R² is a hydrocarbon group having 8 to 22 carbon atoms, ahydrogen atom or a group represented by the formula: (AO)_(m) --Hwherein AO represents an oxyalkylene group having 2 or 3 carbon atoms;and m represents a number of 1 to 30!; R³ is a hydrogen atom or a grouprepresented by the formula: (AO)_(m) --H wherein AO and m are those asthe above definitions!; R⁴ is a hydrogen atom or a group represented bythe formula: (AO)_(m) --H wherein AO and m are those as the abovedefinitions!; A is an ethylene group or a propylene group; and p is aninteger of 2 to 5.

The composition for asphalt emulsion of the tenth embodiment of thepresent invention may further contain (C) at least one member selectedfrom the group consisting of anionic polymeric dispersants,hydroxycarboxylic acids and water-soluble salts of hydroxycarboxylicacids, and/or, (D) at least one member selected from the groupconsisting of saccharides, sugar alcohols and polyhydric alcohols.

Further, the eleventh embodiment of the present invention relates to anasphalt emulsion comprising asphalt, water and the composition forasphalt emulsion of the tenth embodiment of the present invention.

The asphalt emulsion of the eleventh embodiment of the present inventionincludes an asphalt emulsion characterized by containing 0.01 to 10.0parts by weight of (A) one or more surfactant selected from amongaliphatic amines represented by the following formula (1'), aminatedlignins, imidazolines having a hydrocarbon group having 8 or more carbonatoms, betaines having a hydrocarbon group having 8 or more carbon atomsand amidobetaines having a hydrocarbon group having 8 or more carbonatoms and 0.01 to 5.0 parts by weight of (B) a polyphenolic compound,per 100 parts by weight of the total of 40 to 80 parts by weight ofasphalt and 60 to 20 parts by weight of water:

    R.sup.1 R.sup.2 --N--(ANR.sup.3).sub.p R.sup.4             ( 1')

(wherein R¹ : represents a hydrocarbon group or acyl group having 8 to22 carbon atoms,

R² : represents a hydrocarbon group having 8 to 22 carbon atoms or R³,

R³, R⁴ : represents H or (AO)_(m),

AO: represents an oxyalkylene group having 2 to 3 carbon atoms,

m: represents a number of 1 to 30,

A: represents an ethylene group or a propylene group,

p: represents a number of 2 to 5).

Furthermore, the twelfth embodiment of the present invention relates toa paving composition which is used for, e.g., paving a road, comprisingaggregate and the asphalt emulsion of the eleventh embodiment of thepresent invention, wherein the amount of the aggregate is 75 to 95 partsby weight and the amount of the asphalt emulsion is 25 to 5 parts byweight per 100 parts by weight of the total of the aggregate and theasphalt emulsion.

The thirteenth embodiment of the present invention relates to use of thecomposition for asphalt emulsion of the tenth embodiment of the presentinvention for preparing an asphalt emulsion.

The fourteenth embodiment of the present invention relates to acomposition for emulsification which comprises water, (A-1) at least onemember selected from the group consisting of aliphatic aminesrepresented by the above formula (1), aminated lignins, imidazolineshaving a hydrocarbon group having 7 or more, preferably 8 or more,carbon atoms, betaines having a hydrocarbon group having 7 or more,preferably 8 or more, carbon atoms and amidobetaines having ahydrocarbon group having 7 or more, preferably 8 or more, carbon atoms,and (B) a polyphenolic compound.

The composition for emulsification of the fourteenth embodiment of thepresent invention may further contain the above components (C) and (D).

The fifteenth embodiment of the present invention relates to a processfor the preparation of the composition for emulsification of thefourteenth embodiment of the present invention containing components (C)and (D), which comprises step 1 of adding a mixture of component (A-1)and component (D) to an aqueous solution of component (B) to prepare anaqueous solution, and step 2 of adding an aqueous solution of component(C) to the obtained aqueous solution.

The sixteenth embodiment of the present invention relates to a processfor the preparation of the composition for emulsification of thefourteenth embodiment of the present invention containing components (C)and (D) and a monobasic acid, which comprises step 1 of adding amonobasic acid to an aqueous solution of component (B) to prepare anaqueous acidic solution, step 2 of adding a mixture of component (A-1)and component (D) to the aqueous acidic solution to prepare an aqueoussolution, and step 3 of adding an aqueous solution of component (C) tothe obtained aqueous solution.

The seventeenth embodiment of the present invention relates to a processfor emulsifying asphalt in water, which comprises adding molten asphaltto the composition for emulsification of the fourteenth embodiment ofthe present invention to prepare a mixture and then emulsifying themixture.

The eighteenth embodiment of the present invention relates to use of thecomposition for emulsification of the fourteenth embodiment of thepresent invention for emulsifying asphalt.

Further, the scope and application of the present invention will beclarified from the following Detailed Description and Examples. However,it should be understood that the Detailed Description and Examples,which show preferred embodiments of the present invention, are givenonly for explanation, because various alternations and modificationswithin the attempt and scope of the present invention will be apparentto any person skilled in the art from this Detailed Description.

DETAILED DESCRIPTION OF THE INVENTION

Component (A) in the present invention may be any of cationic, nonionic,anionic and amphoteric surfactants. As the emulsifier (A), only one maybe used, or it may be a multicomponent system comprising two or moremembers. For the preparation of an asphalt emulsion for blending, it ispreferable to use at least one member selected from the group consistingof cationic and amphoteric surfactants.

Examples of the anionic surfactants to be used in the present inventioninclude the following ones having one or two hydrophilic groups in themolecule:

(a) sulfate esters of alcohols having 4 to 18 carbon atoms, and saltsthereof,

(b) alkane-, alkene- and alkylaryl-, which have 4 to 18 carbon atoms,sulfonic acids, and salts thereof,

(c) sulfates and phosphate esters of alkylene oxide adducts of compoundshaving at least one active hydrogen in the molecule, and salts thereof,

(d) esters of alcohols having 4 to 22 carbon atoms with sulfosuccinicacid, and salts thereof,

(e) alkyl(C₈ -C₁₈)diphenyl ether disulfonic acids, and salts thereof,

(f) rosin acids (resin acids) and salts thereof, and tall oil mixedacids which are mixed acids of rosin acids with higher fatty acids, andsalts thereof,

(g) alkane- and alkene-, which have 4 to 18 carbon atoms, fatty acids,and salts thereof, and

(h) salts of α-sulfofatty acid esters.

Examples of the cationic surfactants include alkylamine salts,alkanolamines, quaternary ammonium salts, amine oxides andpolyethylenepolyamines, and adducts of these compounds with ethyleneoxide and/or propylene oxide are also included in the examples thereof.

In the present invention, it is preferable to use a cationic surfactantin which the number of nitrogen atoms contained in one molecule is largeas the emulsifier (A), in order to satisfy the performances required inan emulsion for blending containing it, such as mixability withaggregate and easiness of controlling the decomposition time. Such acationic surfactant is highly polar and therefore has high water holdingproperty, so that the asphalt emulsion containing the surfactantexhibits a high stability when mixed with aggregate. It is preferableparticularly in the preparation of an emulsion for blending to use sucha cationic surfactant.

The reasons therefor are as follows. Aggregate to be used for paving aroad has negative charge. Therefore, when an asphalt emulsion comprisinga cationic surfactant comes into contact with the surface of theaggregate, the emulsified particles are electrically neutralized, bywhich the emulsion is broken through aggregation and the asphalt adheresto the surface of the aggregate. When one having a small number ofnitrogens contained in one molecule, such as monoamine salts, diaminesalts and quaternary ammonium salts, is used in the preparation of anemulsion for blending, the stability of the thus-obtained emulsionbecomes unsatisfactory and the break of the emulsion based on the abovemechanism may occur in a short time, in some cases. That is, it isafraid to be caused such the situation that the decomposition time istoo short.

On the other hand, polyamine salts wherein the number of nitrogenscontained in one molecule is 3 or more exhibit high affinity with waterwhich constitutes the continuous phase of an asphalt emulsion, and it isnot decomposed, i.e., the break of the emulsion does not occur, in ashort time, even when it comes into contact with aggregate. Further,after the emulsion is decomposed and the polyamine salt adheres toaggregate, firm adherent property is exhibited since it electricallybonds with the aggregate. Accordingly, such polyamines are desirable asthe surfactant to be used in the preparation of an emulsion forblending.

In the first to ninth embodiments of the present invention, it isparticularly preferable to use an aliphatic amine represented by theabove formula (1) together with a polyphenolic compound (B) or the like.An asphalt emulsion containing such an aliphatic amine and apolyphenolic compound (B) is extremely excellent in mixability withaggregate and the paving executed by the use of such the emulsion hasextremely high strength and endurance. Although the species of thesurfactants to be used is limited to components (A-1) in the tenth toeighteenth embodiments of the present invention, the aliphatic aminerepresented by the above formula (1) is one of components (A-1).

Other preferable examples of the cationic surfactants include aminatedlignins and imidazolines having a hydrocarbon group having 7 or more,preferably 8 or more, still more preferably 8 to 22 carbon atoms. Anasphalt emulsion containing such a cationic surfactant and apolyphenolic compound (B) is extremely excellent in mixability withaggregate and the paving executed by the use of such the emulsion hasextremely high strength and endurance. Although the species of thesurfactants to be used is limited to components (A-1) in the tenth toeighteenth embodiments of the present invention, the aminated lignin andthe imidazoline having a hydrocarbon group having 7 or more carbon atomsare each one of components (A-1).

Among aminated lignins, those represented by the following formula (2)are particularly preferable, while among imidazolines having ahydrocarbon group having 7 or more carbon atoms, those represented bythe following formulae (3) and (4) are particularly preferable: ##STR2##wherein R represents a hydrocarbon group having 7 to 22, preferably 8 to22, carbon atoms, and ##STR3## wherein R represents a hydrocarbon grouphaving 7 to 22, preferably 8 to 22, carbon atoms.

The cationic surfactants other than quaternary ammonium salts are usedin the form of a salt thereof with a monobasic acid such as hydrochloricacid, acetic acid, nitric acid and sulfamic acid.

Examples of the amphoteric surfactants include those of a betaine typeand an amidobetaine type, and phospholipids such as phosphatidylcholine,phosphatidylserine and phosphatidylethanolamine. Among them, betaineshaving a hydrocarbon group having 7 or more, preferably 8 or more, stillmore preferably 8 to 22, carbon atoms, and amidobetaines having ahydrocarbon group having 7 or more, preferably 8 or more, still morepreferably 8 to 22, carbon atoms are desirable for the same reasons asthose in the case of the cationic surfactants.

Among betaines having a hydrocarbon group having 7 or more carbon atoms,those represented by the following formula (5) are particularlypreferable, while among amidobetaines having a hydrocarbon group having7 or more carbon atoms, those represented by the following formula (6)are particularly preferable: ##STR4## wherein R represents a hydrocarbongroup having 7 to 22, preferably 8 to 22, carbon atoms, and ##STR5##wherein R represents a hydrocarbon group having 7 to 22, preferably 8 to22, carbon atoms.

Examples of the nonionic surfactants include polyethylene glycol typesurfactants such as adducts of higher alcohols with ethylene oxide,adducts of alkylphenols with ethylene oxide, adducts of fatty acids withethylene oxide, adducts of polyhydric alcohol/fatty acid esters withethylene oxide, adducts of higher alkylamines with ethylene oxide,adducts of fatty acid amides with ethylene oxide, adducts of fats andoils with ethylene oxide and adducts of polypropylene glycol withethylene oxide; and polyhydric alcohol type surfactants such asglycerol/fatty acid esters, pentaerythritol/fatty acid esters,sorbitol/fatty acid esters, sorbitan/fatty acid esters, sucrose/fattyacid esters, alkyl ethers of polyhydric alcohols and fatty acid amidesof alkanolamines.

It is desirable to use, as the emulsifier (A), one of which the HLB is10 or above.

In the asphalt emulsion according to the present invention, component(A) or (A-1) is used in an amount of preferably 0.01 to 10 parts byweight, still more preferably 0.05 to 3.0 parts by weight, per 100 partsby weight of the total of asphalt and water.

In the polyphenolic compound (B) to be used in the present invention,compounds having hydroxyl groups on an aromatic ring(s) such as benzenering wherein the number of such the hydroxyl groups is two or more perone molecule (which include monocyclic compounds and polycycliccompounds); substance prepared by the oxidative polymerization of suchthe compounds; and the like are included. Specific examples thereofinclude hydrolyzable tannins such as gallnut tannin, nutgalls tannin,sumach tannin, fatsia tannin, valonia tannin, chestnut tannin, myrobalantannin, oak tannin, divi-divi tannin and algarobia tannin; condensedtannins such as gambir tannin, quebracho tannin, mimosa tannin, mangrovetannin, hemlock tannin, Spruce tannin, Burma cutch tannin, oak barktannin and persimmon tannin; tannin compounds such as rice tannin,cascarote tannin, acacia tannin, depside, Chinese tannin, Turkishtannin, hamamelitannin, quebric acid and ellargic acid tannin; purifiedtannic acids originating from these tannin compounds; polyhydric phenolssuch as catechol, resorcinol, hydroquinone, pyrogallol, phloroglucinoland gallic acid; gallic acid derivatives; and lignins. In the additivecomposition for asphalt emulsion of the first embodiment of the presentinvention and an asphalt emulsion and the like using it, it ispreferable to use as component (B) at least one member selected from thegroup consisting of tannin compounds, tannic acid, catechol, resorcinol,hydroquinone, pyrogallol, gallic acid and gallic acid derivatives, andit is still more preferably to use at least one member selected from thegroup consisting of tannin compounds, tannic acid and pyrogallol. While,in the composition for asphalt emulsion of the tenth embodiment of thepresent invention and an asphalt emulsion and the like using it, it ispreferable to use as component (B) at least one member selected from thegroup consisting of tannin compounds, tannic acid, catechol, resorcinol,hydroquinone, pyrogallol, gallic acid and gallic acid derivatives.

In the present invention, as component (B), use can be made them eachalone, or after mixing two or more of them. The use amount thereof ispreferably 0.01 to 10.0 parts by weight, still more preferably 0.1 to3.0 parts by weight per 100 parts by weight of the total of asphalt andwater in the asphalt emulsion of the second embodiment of the presentinvention or the like, and is preferably 0.01 to 5.0 parts by weight,still more preferably 0.03 to 4.0 parts by weight, particularlypreferably 0.05 to 3.0 parts by weight per 100 parts by weight of thetotal of asphalt and water in the asphalt emulsion of the eleventhembodiment of the present invention or the like.

In the present invention, it is preferable to use, as the polyphenoliccompound (B), one wherein the percentage of absolute area of thecomponents having a weight-average molecular weight, on chromatogram, of2800 or above is 10% or below in the molecular weight distribution asdetermined by gel permeation chromatography (GPC) effected afteracetylation thereof. Such a polyphenolic compound can be obtained byfractionating a polyphenolic compound by column chromatography.

The method of acetylating a polyphenolic compound and determining themolecular weight (distribution) of the obtained derivative by GPC is asfollows.

Acetylation Process!

A sample is acetylated according to the description of Kobunshi BunsekiHandbook (Handbook for the analysis of polymers) (pp. 783-784, publishedby Kinokuniya Shoten, 1995). That is, 2 g of a sufficiently dried sampleis put in a 50-ml Erlenmeyer flask fitted with a ground-in glassstopper, and 10 ml of pyridine and 10 ml of acetic anhydride are addedthereto while cooling with ice to dissolve the sample. At the point oftime when the generation of heat is discontinued, the flask is stoppedup and thereafter is allowed to stand at a room temperature (20° C.) ina dark place for 12 hours. Then, the contents of the flask are pouredinto a 200-ml beaker holding 100 ml of ice-water to precipitate anacetylate. After the precipitate is recovered by filtration and washedwith ice-water, it is dried with nitrogen, and then dried in a vacuum atordinary temperatures. Thus, an acetylate is obtained.

Conditions of Determination by GPC!

sample size: 0.5%, 100 ml

column: G4000HXL+G2000HXL (a product of Tosoh Corporation)

eluent: 50 mM CH₃ COOH/THF

flow rate: 1.0 ml/min

column temp.: 40°

detector: R1

ref. material: polystyrene.

As the polyphenolic compound (B), from the standpoint of adherencethereof to aggregate, those wherein the percentage of absolute area ofthe components having a weight-average molecular weight, onchromatogram, of 2800 or above is 10% or below, still more 5% or below,particularly 1% or below, in the molecular weight distribution afteracetylation thereof, are preferable. Further, those wherein thepercentage of absolute area of the components having a weight-averagemolecular weight, on chromatogram, of 1500 to 2600 is 90% or above,particularly 95% or above, in the molecular weight distribution afteracetylation, are preferable. Furthermore, those wherein the ratio(Mw/Mn) of the weight-average molecular weight (Mw) to thenumber-average molecular weight (Mn) is 1.4 or below, still more 1.3 orbelow, particularly 1.2 or below, in the molecular weight distributionafter acetylation, are preferable.

The effects brought about by the addition of the polyphenolic compound(B) to an asphalt emulsion are resulted from such the chemical structurelike a surfactant that such the compound has simultaneously ahydrophobic skeleton and a hydrophilic group (hydroxyl group). By virtueof such the chemical structure, the polyphenolic compound (B) adheres tothe surface of an asphalt particle through wetting and penerationfunctions thereof and forms a protective layer around the asphaltparticle by forming a hydrated structure due to many hydroxyl groups.Thus, the asphalt particles are stabilized in the emulsion, so that theemulsion does not cause rapid decomposition even when mixed withaggregate. Further, aggregate on a wet state has hydroxyl groups on thesurface and, therefore, these hydroxyl groups form hydrogen bondingstogether with the hydroxyl groups of the polyphenolic compound (B). Itis presumed that such hydrogen bondings together with the physicaladsorption of asphalt itself to aggregate make asphalt adhere toaggregate firmly.

In the present invention, at least one member selected from the groupconsisting of anionic polymeric dispersants, hydroxycarboxylic acids andwater-soluble salts of hydroxycarboxylic acids is used as component (C).

Examples of the anionic polymeric dispersants to be used in the presentinvention include naphthalenesulfonic acid/formaldehyde condensate,melaminesulfonic acid/formaldehyde condensate, phenolsulfonicacid/formaldehyde condensate, polycarboxylic acid copolymers andwater-soluble salts thereof, kraut lignins obtained from needle-leavedtrees and broad-leaved trees, ligninsulfonic acids and water-solublesalts thereof, and starches such as tapioca starch. Among them,ligninsulfonic acids and water-soluble salts, such as Na salts, Casalts, Mg salts, Zn salts and Al salts, of ligninsulfonic acids arepreferable.

In the present invention, a hydroxycarboxylic acid or a water-solublesalt thereof may be used as component (C) instead of or together withthese anionic polymeric dispersant. Examples of the hydroxycarboxylicacids include gluconic acid, glucoheptonic acid, arabonic acid, malicacid and citric acid. While, its water-soluble salt means its sodiumsalt or the like. In the present invention, sodium gluconate isparticularly preferably used.

In, e.g., the asphalt emulsion of the second embodiment of the presentinvention, component (C) is used in such an amount that the total ofthis component (C) and component (D) which will be described below ispreferably 0.01 to 10 parts by weight, still more preferably 0.01 to 2.0parts by weight, particularly preferably 0.05 to 2.0 parts by weight per100 parts by weight of the total of asphalt and water. In this case, theamount of component (C) to be used is also preferably 0.01 to 10 partsby weight, still more preferably 0.01 to 2.0 parts by weight,particularly preferably 0.05 to 2.0 parts by weight per 100 parts byweight of the total of asphalt and water. On the other hand, in, e.g.,the asphalt emulsion of the eleventh embodiment of the presentinvention, component (C) is used in an amount of preferably 0.01 to 10parts by weight, still more preferably 0.01 to 2.0 parts by weight,particularly preferably 0.05 to 2.0 parts by weight per 100 parts byweight of the total of asphalt and water. When the amount of component(C) or the total amount of components (C) and (D) is too large, thestorage stability of the asphalt emulsion will be poor in some cases.Component (C) is a substance which has hitherto been used as adispersant for inorganic materials or cement, and it is effective inimproving the mixability and dispersibility of powdered stone, calciumcarbonate and cement which are used as clayey aggregates or fillers.

Component (D) in the present invention is at least one member selectedfrom the group consisting of saccharides, sugar alcohols and polyhydricalcohols.

Examples of the saccharides to be used in the present invention includemonosaccharides and disaccharides such as glucose, maltose, fructose,galactose, saccharose and isomerized saccharides; oligosaccharides suchas dextrin; and polysaccharides such as dextran. Further, molassescontaining them are also included in the saccharides of the presentinvention. An example of the sugar alcohol includes sorbitol. Thepolyhydric alcohol may be any one so long as it has two or more hydroxylgroups in the molecule and is dissolved in water, and examples thereofinclude polyethylene glycol, glycerol, ethylene glycol, propyleneglycol, polyglycerol and diethylene glycol. When polyethylene glycol isused in the present invention, those having an average molecular weightof 200 to 5000 are preferred.

As component (D) which is used in the additive composition for asphaltemulsion of the first embodiment of the present invention and in anasphalt emulsion or a composition for emulsification containing it, atleast one member selected from the group consisting of sorbitol,glycerol and polyethylene glycols having an average molecular weight of200 to 5000 is preferred, at least one member selected from the groupconsisting of sorbitol, glycerol and polyethylene glycols having anaverage molecular weight of 200 to 800 is still more preferred, andglycerol is particularly preferred. On the other hand, as component (D)which is used in the additive composition for asphalt emulsion of thetenth embodiment of the present invention and in an asphalt emulsion ora composition for emulsification containing it, at least one memberselected from the group consisting of maltose, saccharose, sorbitol,glycerol and polyethylene glycols having an average molecular weight of200 to 5000 is preferred, at least one member selected from the groupconsisting of sorbitol, polyethylene glycols having an average molecularweight of 200 to 5000 and glycerol is still more preferred, and apolyethylene glycol having an average molecular weight of 200 to 800 ismost preferred.

In, e.g., the asphalt emulsion of the second embodiment of the presentinvention, component (D) is used in such an amount that the total ofthis component (D) and the above-described component (C) is preferably0.01 to 10 parts by weight, still more preferably 0.01 to 2.0 parts byweight, particularly preferably 0.05 to 2.0 parts by weight per 100parts by weight of the total of asphalt and water. In this case, theamount of component (D) to be used is preferably 0.01 to 10 parts byweight, still more preferably 0.05 to 2.0 parts by weight per 100 partsby weight of the total of asphalt and water. On the other hand, in,e.g., the asphalt emulsion of the eleventh embodiment of the presentinvention, component (D) is used in an amount of preferably 0.01 to 10parts by weight, still more preferably 0.05 to 2.0 parts by weight per100 parts by weight of the total of asphalt and water. When the amountof component (D) or the total amount of components (C) and (D) is toolarge , the adherence of asphalt to aggregate will be poor, so that thestrength and endurance of the paving executed by the use of such theasphalt emulsion will be lowered. In the paving composition, component(D) can hold water which serves as lubricant and therefore is effectivein enhancing the lubricity among solid particles (aggregate). In otherwords, component (D) contributes in the enhancement of the flowabilityin the paving compositions of the third and twelfth embodiments of thepresent invention. Accordingly, when component (D) exists, the mixabiltyof the asphalt emulsion with aggregate can be secured and therefore theworkability of the above paving composition can be kept, even undersevere conditions of high atmospheric temperature.

The additive composition for asphalt emulsion and the composition forasphalt emulsion of the present invention are used in the preparation ofan asphalt emulsion. The additive composition for asphalt emulsion ofthe first embodiment of the present invention comprises components (B),(C) and (D) as essential components and optionally the emulsifier (A).The additive composition for asphalt emulsion is used together with asuitable emulsifier, water and asphalt to give an asphalt emulsion,independent of whether it contains the emulsifier (A) or not.Alternatively, when the additive composition for asphalt emulsioncontains the emulsifier (A), an emulsifier may not be further added inthe preparation of an asphalt emulsion. On the other hand, thecomposition for asphalt emulsion of the tenth embodiment of the presentinvention comprises components (A-1) and (B) as essential components andoptionally component (C) and (D). This composition for asphalt emulsionis used together with water and asphalt to give an asphalt emulsion. Ofcourse, another emulsifier may also be added.

The concepts of the additive composition for asphalt emulsion and thecomposition for asphalt emulsion of the present invention include kitswherein the constituents thereof are packaged respectively, and thelike.

In the preparation of asphalt emulsions, it is preferable to use thecompositions for emulsification of the fifth and fourteenth embodimentsof the present invention, though it is acceptable that the necessarycomponents among components (A) or (A-1)! are respectively dissolved inwater to give aqueous solutions, and asphalt is emulsified by the use ofsuch the aqueous solutions, suitably. In these compositions foremulsification, all of the components except asphalt among theconstituents of an asphalt emulsion can be contained and, therefore,asphalt emulsions can easily be prepared by the use of thesecompositions. When these compositions for emulsification contain acationic surfactant such as amine-type ones, the compositions foremulsification may contain, in some cases, a monobasic acid which makesit to be an acid-type one.

The composition for emulsification can be prepared by adding thecomponents to water successively or by preliminary preparing a mixtureof the components to be added to water and adding the mixture to water.When a cationic surfactant other than quaternary ammonium salt typesurfactants and/or an amphoteric surfactant is used as the emusifier (A)or (A-1)!, it is preferable that the compositions for emulsification areprepared by the processes of the sixth, seventh, fifteenth and sixteenthembodiment of the present invention as described above.

Still more preferable examples of the processes for preparing thecomposition for emulsification of the present invention include aprocess procedure (1)! which comprises

(1) preparing an aqueous solution of component (B),

(2) adding a monobasic acid such as hydrochloric acid to the aqueoussolution of component (B),

(3) adding a separately prepared mixture comprising component (D) and acationic surfactant and/or an amphoteric surfactant component (A) or(A-1)! to the aqueous solution prepared in step (2), and

(4) adding a separately prepared aqueous solution of component (C) tothe aqueous solution prepared in step (3);

and a process procedure (2)! which comprises

(1) preparing an aqueous solution containing components (B) and (C),

(2) adding a monobasic acid such as hydrochloric acid to the aqueoussolution prepared in step (1), and

(3) adding a separately prepared mixture comprising component (D) and acationic surfactant and/or an amphoteric surfactant component (A) or(A-1)! to the aqueous solution prepared in step (2). The temperatureswhen these processes are conducted are preferably 60 to 80° C. Further,the composition for emulsification preferably has a solid content of 40to 60% by weight.

When the composition for emulsification is prepared by such the process,a homogeneous and one solution type composition can be obtained. In theabove procedures (1) and (2), item (2) may be dispensed, depending uponthe kind of the surfactant used. Although the particularly properselection between the above procedures (1) and (2) is unnecessary, theemployment of the procedure (1) is preferable in the case where a solidsurfactant which can be converted into liquid by changing the conditionssuch as temperature and concentration, for example, an adduct of a solidamine with an alkylene oxide, is used as the emulsifier (A) or (A-1)!.While, the employment of the procedure (2) is preferable in the casewhere the emulsifier (A) or (A-1)! is a solid one which is difficult ofmixing with water, for example, a tallow-alkyl dialkylenetriamine. Whena nonionic surfactant, an anionic surfactant or a quaternary ammoniumsalt type surfactant is used as the emulsifier (A) or (A-1)! instead ofor together with the cationic surfactant and/or the anionic surfactant,it may be added in any step in the procedures (1) and (2).

Further, it is preferable to prepare a composition for emulsificationcomprising components (A), (B) and (C) by a process comprising step 1 ofadding component (A) to an aqueous solution of component (B) to preparean aqueous solution and step 2 of adding an aqueous solution ofcomponent (C) to the obtained aqueous solution, or a process comprisingstep 1 of adding a monobasic acid to an aqueous solution of component(B) to prepare an aqueous acidic solution, step 2 of adding component(A) to the aqueous acidic solution to prepare an aqueous solution, andstep 3 of adding an aqueous solution of component (C) to the obtainedaqueous solution.

Furthermore, it is preferable to prepare a composition foremulsification comprising components (A), (B) and (D) by a processcomprising the step of adding a mixture of component (A) and component(D) to an aqueous solution of component (B) to prepare an aqueoussolution, or a process comprising step 1 of adding a monobasic acid toan aqueous solution of component (B) to prepare an aqueous acidicsolution and step 2 of adding a mixture of component (A) and component(D) to the aqueous acidic solution to prepare an aqueous solution.

Examples of the asphalts to be used in the present invention includepetroleum straight asphalt, semi-blown asphalt, cut-back asphalt andnatural asphalt. One of them or a mixture of two or more of them is usedin the preparation of an asphalt emulsion of the present invention.

The asphalt emulsion can be prepared by emulsifying asphalt in one ofthe aqueous solutions respectively containing necessary components amongthe above components (A) or (A-1)!, (B), (C) and (D) or an aqueoussolution (for example, the composition for emulsification according tothe present invention) containing all of such the necessary components.Some of the components are used not in the form of an aqueous solutionthereof but as such. For example, the polyphenolic compound (B) may bepreliminarily dissolved in an aqueous solution of the emulsifier (A) ormay be added in the form as it is to an asphalt emulsion prepared byemulsifying asphalt in an aqueous solution of the emulsifier (A).Although the asphalt emulsion can be prepared only with the waterresulting from the aqueous solutions in some cases, the asphalt emulsionmay be prepared by further adding water at need. In the asphalt emulsionof the second embodiment of the present invention, the weight ratio ofasphalt to water (asphalt/water) is preferably 35 to 90/65 to 10. In theasphalt emulsion of the eleventh embodiment of the present invention,the weight ratio of asphalt to water (asphalt/water) is preferably 40 to80/60 to 20.

The asphalt emulsion of the present invention may further contain anatural rubber, a synthetic rubber such as a styrene-butadienecopolymer, a styrene-isoprene copolymer and a chloroprene copolymer; apolymer such as polyethylene and ethylene-vinyl acetate copolymer; apetroleum resin, a thermoplastic resin or the like. In some case, thesecomponents may be preliminarily mixed with asphalt. Such mixtures arecalled modified asphalts. The asphalt emulsion may further contain also,e.g., inorganic and organic fillers such as calcium carbonate, slakedlime, cement and activated carbon; petroleum softening agents; vegetableoil softening agents, various plasticizers, sulfur and the like.

The paving of a road or the like is conducted by the use of a pavingcomposition comprising the asphalt emulsion and aggregate.

The concept of aggregate to be used in the present invention includesnatural aggregates such as fillers, crushed stone, crushed gravel,gravel, sand and reclaimed aggregates; and artificial aggregates such ascalcined bauxite, special hard slags obtained as by-products in smeltingmetals or non-metals, fused alumina and various abrasive materials. Theconcept of aggregate further includes also tint aggregates which arewhite aggregates prepared by firing natural aggregates or artificialaggregates; and colored aggregates prepared by adding inorganic pigmentsthereto.

The filler has a concept which refers a powdered stone of limestone origneous rock, cement, slaked lime, fly ash or the like.

The crushed stone is a material produced by crushing raw rockmechanically and, if necessary, subjecting the obtained particles tosize classification. The raw rock herein is an igneous rock, asedimentary rock or a metamorphic rock. The igneous rocks are classifiedinto basalt, andesite, liparite, diabase, quartz porphyry, hankigan,diorite, granite and the like, based on the state of deposit and silicacontent. The concept of sedimentary rocks includes tuff, agglomerate,conglomerate, shale, limestone and the like, while that of metamorphicrocks includes mylonite, hornfels, gneiss, crystalline schist and thelike.

The crushed gravel is a material produced by crushing cobble stone orgravel, while the concept of gravel includes river gravel, pit gravel,beach gravel and the like.

The sands are classified into natural sands, artificial sands,screenings, special sands and the like. The natural sands are classifiedinto river sand, pit sand, beach sand and the like, based on the placewhere it was collected. The artificial sand is a material produced bycrushing rock or cobble stone, while the screenings refers to finematerial having a particle diameter of 2.36 mm or below which isobtained in the production of crushed stone or crushed gravel. Theconcept of special sand includes silica sand, water-crushedblast-furnace slag, clinker ash and the like.

The concept of reclaimed aggregate includes reclaimed aggregate ofasphalt concrete produced by the mechanical crushing or thermal crackingof material originating in asphalt concrete pavement, and reclaimedaggregate of cement concrete produced by the mechanical crushing ofmaterial originating in cement concrete pavement. To these reclaimedaggregates, an auxiliary material or an additive for reclamation isadded at need.

The ferrous slag is one prepared by crushing a slag produced in theproduction process of iron and steel. It is classified intoblast-furnace slag obtained from a blast furnace by smelting in theproduction process of pig iron, and steel-making slag produced in theproduction process of steel. In general, hydraulic ferrous slag ofcontrolled grading, ferrous slag of controlled grading, crusher-runferrous slag or the like is used for paving a road.

In the present invention, the weight ratio of aggregate to asphaltemulsion (aggregate/asphalt emulsion) is preferably 75 to 95/25 to 5.

In the preparation of the paving composition which is used for, e.g.,paving a road and which comprises the asphalt emulsion and aggregate, atleast one member selected from the group consisting of water-solubleinorganic salts such as ammonium chloride, potassium chloride, sodiumchloride, calcium chloride, aluminum chloride and iron chloride;water-soluble polymers such as polyvinyl alcohol, gelatin,hydroxyethylcellulose, methylcellulose and cationic starch; andwater-soluble natural rubbers may further be used, depending upon theuse and object of the composition, the method of execution or the like.Further, water may further be added when water is unsufficiet by the useof only the water resulting from the asphalt emulsion.

As described above in detail, according to the present invention, anasphalt emulsion satisfying all of the properties required in themarket, for example, storage stability, mixability with aggregate andanti-foaming properties of the emulsion itself, adherence of theproducts of breaking of the emulsion to aggregate, stripping resistanceof the construction executed by the use of the emulsion and so on, canbe provided. Particularly when an asphalt emulsion wherein a specificemulsifier is used is employed, there are excellent further inmixability with cement and easiness of controlling the decompositiontime of the emulsion itself, adherence of the products of breaking ofthe emulsion to crushed stone, and strength and endurance of theconstruction (such as paving of a road) executed by the use of theemulsion.

Such the asphalt emulsion can effectively be used in the uses such asthe paving of a road, the construction of railway, cement asphaltmortar, corrosion prevention, rust prevention, waterproofing, bonding,agricultural land reclamation and so on.

EXAMPLES

The present invention will be illustrated in more detail by referring tothe following Examples, though it should not be considered that theExamples limit the scope of the present invention.

Examples 1 to 9 and Comparative Examples 10 to 17

Preparation of Asphalt Emulsion!

An asphalt having a penetration of 80 to 100 was heated to 145° C. tomelt.

Separately, components which would be added to an asphalt emulsionlisted in Table 1 or 2 were dissolved in warm water at 45° C. to preparean aqueous solution. 40 parts by weight of the thus-prepared aqueoussolution for emulsification of 45° C. and 60 parts by weight of a moltenasphalt of 145° C. were simultaneously passed through a barrel typehomogenizer to prepare an asphalt emulsion. Only when an amine typesurfactant (i.e., tallow-alkyl propylenediamine) was used, the pH of theaqueous solution for emulsification was adjusted to 2 by usinghydrochloric acid.

With respect to the asphalt emulsions thus prepared, the storagestability, mixability with cement and mixability with aggregate, and theadherence of the products of breaking thereof to crushed stone wereexamined. The results are given in Tables 1 and 2. The testing methodsare those as will be described below.

Testing Methods!

(1) Storage stability of emulsion

The storage stability of an emulsion was examined according to JIS K2208 (1980). Specifically, the experiment was conducted as follow.

1) 250 ml of a sample is weighed into a cylinder having an innerdiameter of 32 mm and a height of 340 mm and fitted with two samplingports on the side; and the cylinder is stopped up and allowed to standas such at room temperatures for 5 days.

2) About 50 g of the sample is taken out through the upper sampling portA without shaking the cylinder, followed by accurate weighing.

3) The sample present between the sampling ports A and B is dischargedthrough the lower sampling port B.

4) The sample remaining at the bottom of the cylinder is stirred; andthen about 50 g of the sample is taken out through the sampling port B,followed by accurate weighing.

5) The samples taken out in steps 2) and 4) are each heated for 20 to 30minutes.

6) After the disappearance of water has been confirmed, the samples arefurther heated at 160° C. for one minute and thereafter cooled to roomtemperature by allowing to stand,

7) The percentage by mass (referred to as evaporation residue) of theresidue (g) of the evaporation based on the sample (g) is determined.

8) The difference between the evaporation residues of both samples iscalculated.

In Tables, together with the values determined, the cases where it meetsthe standard requirement, i.e., those where the difference between thenumerical values of the evaporation residues is 5% or below, are shownby the symbol ∘, and those where it does not meet are shown by thesymbol X.

(2) Mixability with cement

The mixability of an emulsion with cement was examined according to ASTMD244 33-37. Specifically, the experiment was conducted as follows.

1) A sample is diluted with distilled water to such an extent that theresidue of distillation or 3-hour evaporation at 163° C. is 55%.

2) 50 g of cement passing through a No.80 sieve (180 μm) is put in adish or saucepan made of iron.

3) 100 ml of the diluted sample is added to the cement; and immediatelythereafter, the obtained mixture is stirred at 60 rpm by the use of astirring rod.

4) One minute after the initiation of the stirring, 150 ml of distilledwater is added; and the obtained mixture is stirred for 3 minutes. Steps3) and 4) are conducted at 25° C. throughout.

5) The obtained mixture is poured onto a No. 14 sieve (1.40 mm). Themixture adhering to the vessel is also poured thereonto completely bywashing the vessel with the filtrate repeatedly.

6) The cake on the sieve is sufficiently washed with distilled water.

7) The cake on the sieve is heated at 163° C.

8) The weight (g) at the point of time when the change in weight byheating becomes 0.1 g or below is regarded as the residue (%) ofemulsion breaking in the cement mixture test.

In Tables, together with the values determined, the cases where it meetsthe standard requirement, i.e., those where it is 2% or below, are shownby the symbol ∘, and those where it does not meet are shown by thesymbol X.

(3) Adherence to crushed stone

Dry crushed stones having a diameter of 5 to 13 mm were dipped in waterfor one minute. Immediately after being taken out of the water, thecrushed stones were dipped in an emulsion for one minute. The crushedstones taken out of the emulsion were placed in order on a glass plateand aged as such at room temperatures for 24 hours. After aging, theresulting crushed stones were immersed in warm water at 80° C. for onehour. One hour after they were taken out of the warm water, the ratiosof areas of the asphalt films covered on the surfaces of the crushedstones were evaluated by the naked eye and the ratios were regarded asthe ratios (%) of adhered areas. Herein, the number of the crushedstones used in one test was ten and the kind of the stones waslimestone.

In Tables, the average values of the ratios (%) of asphalt-adhered areasof ten crushed stones and the results of evaluation made according tothe following criteria are given.

X: the ratio of asphalt-adhered area is less than 50%,

Δ: the ratio of asphalt-adhered area is 50% or above but below 70%,

∘: the ratio of asphalt-adhered area is 70% or above but below 90%, and

⊚: the ratio of asphalt-adhered area is 90% or above.

(4) Mixability with aggregate

60 g of additive water was added to 2200 g of dry aggregate which meetsa particle size distribution of aggregate for dense grade mixture asdescribed in Outlines for Paving a Road, i.e., has a particle sizedistribution which will be described in the following Table A. Theobtained mixture was agitated, and then 240 g of an asphalt emulsion wasadded thereto. The mixture thus obtained was kneaded for 2 minutes, andthe mixability of the asphalt emulsion with the aggregate was evaluatedaccording to the following criteria. The testing temperature(temperature at evaluation) was 25° C., and in mixing, a mixer(capacity: 5 l) for preparation of asphalt mixture mfd. by World Test(K.K.) was used.

The results of evaluation according to the following criteria are givenin Tables.

X: the emulsion was decomposed (i.e., the emulsion was broken) duringkneading,

Δ: they were uniformly mixed, but immediately thereafter the emulsionwas decomposed,

∘: they were uniformly mixed, but the working life of the emulsion (thetime until the breaking of the emulsion) was short, and

⊚: they were uniformly mixed, and the emulsion had a sufficiently longworking life and a good workability.

                  TABLE A    ______________________________________    Max. particle size mm                         20    ______________________________________    Percentage     26.5   mm     100    by mass of     19     mm      95˜100    undersize      13.2   mm     75˜90    %              4.75   mm     45˜65                   2.36   mm     35˜50                   600    μm  18˜30                   300    μm  10˜21                   150    μm   6˜16                   75     μm  4˜8    ______________________________________

                  TABLE 1    ______________________________________    Additives             Ex.    (pts. by wt.)             1      2      3    4    5   6    7   6    9    ______________________________________    Component    (A)    alkyl(C.sub.18)tri-             0.5    0.5                       0.5    methyl    ammonium    chloride    tallow-alkyl           0.5           0.2      0.5  0.5    propylene-    diamine*    polyoxy-                    0.3  0.3    ethylene    (PEO = 50)    nonylphenyl    ether    aminated lignin             0.3      0.4           0.2    sodium                           0.3    dodecyl-    benzenesulfate    Component    (B)    pyrogallol             0.3                                  0.1    tanninc acid    0.3                  0.1  0.3      0.1    (reagent)    quebracho              0.3  0.3  0.3 0.1      0.1    tannin    Component    (C)    calcium  0.2    0.2         0.1           0.1 0.2  0.1    ligninsulfonate    sodium                 0.2       0.1               0.1    gluconate    Component    (D)    glycerol                                  0.1      0.1    polyethylene                                  0.1    glycol    (Mw = 600)    sorbitol                             0.2           0.1    Total Amt.**             1.0    1.0    1.0  1.0  1.0 1.0  1.0 1.0  1.0    (pts. by wt.)    of components    (A) to (D)    Results of    examinations    storage  ◯                    ◯                           ◯                                ◯                                     ◯                                         ◯                                              ◯                                                  ◯                                                       ◯    stability of             1.9    1.9    1.1  1.7  1.4 0.2  1.5 0.6  0.7    emulsion    mixability with             ◯                    ◯                           ◯                                ◯                                     ◯                                         ◯                                              ◯                                                  ◯                                                       ◯    cement   0.9    0.9    1.2  0.8  0.1 0.8  0.5 1.2  0.9    adherence to             ⊚                    ⊚                           ⊚                                ⊚                                     ⊚                                         ⊚                                              ⊚                                                  ⊚                                                       ⊚    crushed stone             100    100    100  100  95  100  95  100  95    mixability with             ◯                    ◯                           ◯                                ◯                                     ◯                                         ◯                                              ⊚                                                  ⊚                                                       ⊚    aggregate    ______________________________________     notes)     *tallow alkylNHCH.sub.2 CH.sub.2 CH.sub.2 NH.sub.2     **this is an amount on the basis of the sum total of asphalt and water     being 100 parts by weight.

                  TABLE 2    ______________________________________    Additives      Comp. Ex.    (pts. by wt.)  10     11    12  13  14  15  16   17    ______________________________________    Component (A)    alkyl(C.sub.18)trimethylammonium                   1.5                      0.5    chloride    tallow-alkyl          1.5   0.4             0.5  0.3    propylenediamine*    polyoxyethylene(PEO = 50)   0.3                  0.2    nonylphenyl ether    aminated lignin             0.3 1.0    sodium                              0.5    dodeoylbenzenesulfate    Component (B)    pyrogallol    tanninc acid (reagent)                  0.5      0.3    quebracho tannin                            0.5  0.2    Component (C)    calcium ligninsulfonate             0.5    sodium gluconate    Component (D)    glycerol    polyethylene glycol         0.5    (Mw = 600)    sorbitol    Total Amt.** (pts. by wt.)                   1.5    1.5   1.5 1.0 1.0 1.0 1.0  1.0    of components (A) to (D)    Results of    examinations    storage        X      ◯                                ◯                                    X   ◯                                            X   ◯                                                     ◯    stability of   10.2   1.4   0.9 8.6 3.0 7.9 3.1  4.6    emulsion    mixability with                   ◯                          X     X   X   ◯                                            X   X    X    cement         1.0    8.9   6.7 6.9 1.2 3.0 10.1 7.8    adherence to   X      X     X   Δ                                        X   ◯                                                ◯                                                     X    crushed stone  45     45    30  60  10  80  80   50    mixability with                   X      X     X   X   X   X   X    X    aggregate    ______________________________________     notes)     *tallow alkylNHCH.sub.2 CH.sub.2 CH.sub.2 NH.sub.2     **this is an amount on the basis of the sum total of asphalt and water     being 100 parts by weight.

As is apparent from Tables 1 and 2, Examples of the present inventionwere excellent in mixability with cement and mixability with aggrigate,and with respect to also the adherence of asphalt to crushed stone whichhas an influence on the endurance of paving a road, they exhibitedexcellent performances. The above tests were made on a dense grademixture system having a small amount of the additive water. However, itis considered that excellent mixability was attained in Examples due tothe synergistic action of components (A) to (D), even under such severeconditions. With respect to particularly the mixability with aggregate,the effects were excellent when all of components (A) to (D) were used(Examples 7 to 9).

On the other hand, the systems (Comparative Examples 10, 11 and 13)containing only component (A) (emulsifiers), and the systems(Comparative Examples 12 and 14 to 17) containing only two components,i.e., component (A) and, component (B) (polyphenolic compounds), (C)(anionic polymeric dispersants) or (D) (saccharides), were inferior toExamples in mixability with aggregate. Further, Comparative Examples 11to 13 and 15 to 17 among Comparative Examples described above wereapparently inferior to Examples in the evaluation result of "mixabilitywith cement" which serves as an indication of the mixability of asphaltemulsion with aggregate (particularly the finely powdered or clayeyone). Furthermore, in Comparative Examples 10 to 12, 14 and 17, onlysuch the result that they were inferior to Examples also in adherence tocrushed stone could obtained.

As described above, Examples of the present invention are those capableof satisfying all of the performances including stability of emulsion,mixability with cement, adherence to crushed stone and mixability withaggregate.

Examples 101 to 132 and Comparative Examples 101 to 134

Preparation of Asphalt Emulsion!

Asphalts having penetrations of 60 to 80, 80 to 100 and 150 to 200respectively were each heated to 155° C. to melt.

Separately, a surfactant listed in any of Tables 3 to 12 and calciumchloride were dissolved in warm water at 55° C., and then the componentsother than the surfactant listed in any of Tables 3 to 12 were addedthereto and dissolved therein. 40 parts by weight of the thus-preparedaqueous solution for emulsification of 55° C. and 60 parts by weight ofa molten asphalt of 155° C. were simultaneously passed through a colloidmill to prepare an asphalt emulsion. The amount (unit: part by weight)of each component per 100 parts by weight of this asphalt emulsion wasgiven in Tables 3 to 12. Further, the calcium chloride was used in anamount of 0.15 part by weight per 100 parts by weight of asphaltemulsion. When a cationic surfactant was used, the pH of the aqueoussolution for emulsification was adjusted to 2 by using hydrochloricacid.

With respect to the asphalt emulsions thus prepared, the storagestability, mixability with cement, mixability with aggregate anddecomposition time, and the adherence of the products of breakingthereof to crushed stone were examined. The results are given in Tables3 to 12. The testing methods are those as will be described below.

Testing Methods!

(1) Storage stability of emulsion

The storage stability of an emulsion was examined according to ASTM D24429-32. Specifically, the experiment was conducted as follow.

1) 500 ml of a sample is weighed into a cylinder having an outerdiameter of 50 mm and a capacity of 500 ml; and the cylinder is stoppedup and allowed to stand as such at room temperatures for 5 days.

2) About 55 ml of the sample is pipetted from the top of the cylinderwithout shaking the cylinder, and about 50 g thereof is put in a beakerhaving a capacity of 1000 ml.

3) The sample is heated in an oven at 163±28° C. for 2 hours toevaporate the water contained in the sample.

4) The weight (g) of the residue of the evaporation is determined, andthe percentage by mass (referred as to evaporation residue) of theresidue of the evaporation (g) based on the sample (g) is calculated.

5) About 390 ml of the sample is pipetted from the top of the cylinder.

6) The sample remaining at the bottom of the cylinder is sufficientlystirred, and thereafter about 50 g of the sample is taken out of thecylinder and puts in a beaker having a capacity of 1000 ml.

7) The operations of 3) and 4) are conducted.

8) The difference between the evaporation residues of both samples iscalculated.

In Tables, together with the values determined, the cases where it meetsthe standard requirement, i.e., those where the difference between thenumerical values of the evaporation residues is 5% or below, are shownby the symbol ∘, and those where it does not meet are shown by thesymbol X.

(2) Adherence to crushed stone

The examination and evaluation were conducted in the same manner asthose in Examples 1 to 9.

(3) Mixability with aggregate

The examination and evaluation were conducted in the same manner asthose in Examples 1 to 9. The dry aggregate used herein which meets aparticle size distribution of aggregate for dense grade mixture had suchthe composition that No.6 crushed stone was 34% by weight, No.7 crushedstone was 21% by weight, screenings was 17% by weight, coarse sand was12% by weight, fine sand was 10% by weight and powdered stone was 6% byweight.

(4) Mixability with cement

The examination and evaluation were conducted in the same manner asthose in Examples 1 to 9.

(5) Decomposition time of emulsion

Additive water and an asphalt emulsion were added to aggregate under thesame conditions as those employed in the above test on mixability withaggregate, followed by mixing. After the completion of the mixing, theobtained mixture was allowed to stand under the conditions of 25° C. andrelative humidity of 30%. The state of the mixture was observed with thenaked eye and evaluated according to the following criteria.

X: the emulsion was decomposed in the standing time of below 10 minutes,

Δ: the emulsion was decomposed in the standing time of 10 minutes orabove but below 60 minutes, or that of 10 hours or above,

∘: the emulsion was decomposed in the standing time of 60 minutes orabove but below 2 hours, or that of 6 hours or above but below 10 hours,and

⊚: the emulsion was decomposed in the standing time of 2 hours or abovebut below 6 hours.

Further, with the use of the above asphalt emulsions, the asphaltemulsion composite materials were prepared as that which will bedescribed below, and the radial compression strength test was conductedby using them. The results are given in Tables 3 to 12. The testingmethod are those as will be described below.

Preparation Method of Asphalt Emulsion Composite Material!

10 parts by weight of an asphalt emulsion was mixed with 90 parts byweight of an aggregate having such a composition that No. 6 crushedstone was 34% by weight, No.7 crushed stone was 21% by weight,screenings was 17% by weight, coarse sand was 12% by weight, fine sandwas 10% by weight and powdered stone was 6% by weight, to prepare amixture. 1250 g of the mixture thus obtained was packed into a mold formeasuring Martial stability. The mixture was tamped 75 times, the moldwas reversed and the mixture was further tamped 75 times to prepare anasphalt emulsion composite material.

Testing Method for Radial Compression Strength!

The asphalt emulsion composite material prepared by the above method wastaken out of the mold. After aging at 60° C. for 3 days, it was immersedin warm water at 60° C. for 24 hours. The composite material was takenout of the warm water and cooled to 20° C., and thereafter the radialcompression strength was measured with a load measuring device.

                  TABLE 3    ______________________________________              Ex.              101  102    103    104  105  106  107    ______________________________________    Component A-1    tallow-     0.5    dipropylenetriamine*    tallow-            0.5    tripropylenetetramine*    tallow-tetra-             0.5    propylenepentamine*    tallow-penta-                  0.5    propylenehexamine*    adduct of                           0.6    tallow-dipropylene    triamine with EO    (n = 15)*    adduct of                                0.6    tallow-tripropylene    tetramine with EO    (n = 10)*    adduct of                                     0.6    tallow-tripropylene-    tetramine with PO    (n = 10)*    adduct of    tallow-tetrapro-    pylenepentamine with    PO (n = 7)*    tallow-    alkanoyldiethylene-    triamine**    aminated lignin    stearylimidazoline    laurylbetanine    Component B    gallnut tannic acid                0.3    quebracho tannic acid                       0.3    catechol                  0.5    resorcinol                     0.5    hydroquinone                        0.5    pyrogallol                               0.4    gallic acid                                   0.3    methyl gallate    Components C and D    calcium    ligninsulfonate    sodium gluconate    polyethylene glycol    (MW = 400)    glycerol    sorbitol    Penetration of asphalt    (1/10 mm)    60-80       ◯      ◯  ◯    80-100             ◯    ◯    150-200                   ◯  ◯    Results of    examinations    radial compression                4.2    4.2    3.5  3.8  3.6  4.0  4.2    strength (kgf/cm.sup.2)    storage stability of                ◯                       ◯                              ◯                                   ◯                                        ◯                                             ◯                                                  ◯    emulsion    2.5    1.5    1.7  1.7  2.5  1.7  1.9    adherence to crushed                ⊚                       ⊚                              ⊚                                   ⊚                                        ⊚                                             ⊚                                                  ⊚    stone    mixability with                ◯                       ◯                              ◯                                   ◯                                        ◯                                             ◯                                                  ◯    aggregate    mixability with cement                ◯                       ◯                              ◯                                   ◯                                        ◯                                             ◯                                                  ◯                1.1    1.2    1.2  1.1  1.0  1.0  1.1    decompn. Time of                ◯                       ◯                              ◯                                   ◯                                        ◯                                             ◯                                                  ◯    emulsion    ______________________________________     notes:     *a compound wherein a tallow alkyl group is bonded mainly to the terminal     nitrogen atom (the same applies also to the following Tables).     **the tallowalkanoyl group is bonded mainly to the terminal nitrogen atom     (the same applies also to the following Tables).

                  TABLE 4    ______________________________________              Ex.    Additives (pts. by wt.)                106    109    110  111  112  113  114    ______________________________________    Component A-1    tallow-                                  0.5    dipropylenetriamine    tallow-                                       0.2    tripropylenetetramine    tallow-tetra-    propylenepentamine    tallow-penta-    propylenehexamine    adduct of    tallow-dipropylene-    triamine with EO    (n = 15)    adduct of    tallow-tripropylene                      0.2    tetramine with PO    (n = 10)    adduct of                                     0.3    tallow-tripropylene-    tetramine with EO    (n = 10)    adduct of   0.6    tallow-tetrapro-    pylenepentanine with    PO (n = 7)    tallow-            0.5    alkanoyldiethylene-    triamine    aminated lignin           1.0    stearylimidazoline             0.6    laurylbetanine                      0.7    Component B    gallnut tannic acid       0.1  0.2  0.1  0.2  0.1    quebracho tannic acid                       0.2    0.2    catechol           0.1         0.2    resorcinol                          0.3    hydroquinone                             0.2    pyrogallol                                    0.3    gallic acid    methyl gallate                0.5    Components C and D    calcium    ligninsulfonate    sodium gluconate    polyethylene glycol    (MW = 400)    glycerol    sorbitol    Penetration of asphalt    (1/10 mm)    60-80                          ◯  ◯    80-100      ◯                       ◯    ◯    150-200                   ◯  ◯    Results of    examinations    radial compression                3.7    3.9    4.0  4.1  3.7  4.1  4.2    strength (kgf/cm.sup.2)    storage stability of                ◯                       ◯                              ◯                                   ◯                                        ◯                                             ◯                                                  ◯    emulsion    3.0    3.2    3.1  3.5  2.5  1.8  2.0    adherence to crushed                ⊚                       ⊚                              ⊚                                   ⊚                                        ⊚                                             ⊚                                                  ⊚    stone    mixability with                ◯                       ◯                              ⊚                                   ◯                                        ◯                                             ◯                                                  ◯    aggregate    mixability with cement                ◯                       ◯                              ◯                                   ◯                                        ◯                                             ◯                                                  ◯                1.2    1.1    1.0  1.2  1.2  1.1  1.2    decompn. time of                ◯                       ◯                              ◯                                   ◯                                        ◯                                             ◯                                                  ◯    emulsion    ______________________________________

                  TABLE 5    ______________________________________              Ex.    Additives (pts. by wt.)                115    116    117  118  119  120  121    ______________________________________    Component A-1    tallow-    dipropylenetriamine    tallow-                             0.4  0.3    tripropylenetetramine    tallow-tetra-                0.2    propylenepentamine    tallow-penta-      0.2    propylenehexamine    adduct of    tallow-dipropylene-    triamine with EO    (n = 15)    adduct of   0.2           0.3  0.3            0.3    tallow-tripropylene-    tetramine with EO    (n = 10)    adduct of    tallow-tripropylene-    tetramine with PO    (n = 10)    adduct of          0.3    tallow-tetrapro-    pylenepentamine with    PO (n = 7)    tallow-    alkanoyldiethylene-    triamine    aminated lignin           0.2            0.3  0.1    stearylimidazoline                  0.2    laurylbetanine                 0.1            0.1    Component B    gallnut tannic acid                0.2    0.2    quebracho tannic acid     0.2  0.2  0.2  0.3  0.1    catechol    resorcinol                          0.2    hydroquinone              0.1    pyrogallol                               0.1    gallic acid 0.1    methyl gallate     0.3                        0.3    Components C and D    calcium    ligninsulfonate    sodium gluconate    polyethylene glycol    (MW = 400)    glycerol    sorbitol    Penetration of asphalt    (1/10 mm)    60-80              ◯    ◯    80-100      ◯ ◯  ◯    150-200                        ◯  ◯    Results of    examinations    radial compression                4.3    4.0    4.2  4.1  3.8  4.3  4.1    strength (kgf/cm.sup.2)    storage stability of                ◯                       ◯                              ◯                                   ◯                                        ◯                                             ◯                                                  ◯    emulsion    2.0    3.5    1.5  1.5  2.7  2.5  1.8    adherence to crushed                ⊚                       ⊚                              ⊚                                   ⊚                                        ⊚                                             ⊚                                                  ⊚    stone    mixability with                ◯                       ◯                              ⊚                                   ◯                                        ◯                                             ⊚                                                  ⊚    aggregate    mixability with cement                ◯                       ◯                              ◯                                   ◯                                        ◯                                             ◯                                                  ◯                1.4    1.1    0.9  1.2  1.2  1.0  1.0    decompn. time of                ◯                       ◯                              ◯                                   ◯                                        ◯                                             ◯                                                  ◯    emulsion    ______________________________________

                  TABLE 6    ______________________________________              Ex.    Additives (pts. by wt.)                122    123    124  125  126  127  128    ______________________________________    Component A-1    tallow-                   0.5    dipropylenetriamine    tallow-                        0.4    tripropylenetetramine    tallow-tetra-    propylenepentamine    tallow-penta-    propylenehexamine    adduct of                           0.5    tallow-dipropylene    triamine with EO    (n = 15)    adduct of          0.4                        0.3    tallow-tripropylene-    tetramine with EO    (n = 10)    adduct of                                0.5    tallow-tripropylene-    tetramine with PO    (n = 10)    adduct of    tallow-tetrapro-    pylenepentanine with    PO (n = 7)    tallow-     0.3    alkanoyldiethylene-    triamine    animated lignin                0.3    stearylimidazoline    laurylbetanine                                0.1    Component B    gallnut tannic acid                      0.3    quebracho tannic acid                       0.2                        0.3    catechol                  0.1    resorcinol                     0.1    hydroquinone                        0.2    pyrogallol  0.2                0.3    gallic acid 0.1    0.2    0.2       0.1    methyl gallate    Components C and D    calcium            0.2                        0.1    ligninsulfonate    sodium gluconate          0.2    polyethylene glycol            0.1            0.1    (MW = 400)    glycerol                            0.3    sorbitol                                 0.3    Penetration of asphalt    (1/10 mm)    60-80              ◯    ◯    80-100      ◯ ◯  ◯    150-200                        ◯  ◯    Results of    examinations    radial compression                3.7    4.2    3.9  3.8  4.2  3.9  4.1    strength (kgf/cm.sup.2)    storage stability of                ◯                       ◯                              ◯                                   ◯                                        ◯                                             ◯                                                  ◯    emulsion    3.9    1.5    3.8  1.9  1.5  2.4  1.4    adherence to crushed                ⊚                       ⊚                              ⊚                                   ⊚                                        ⊚                                             ⊚                                                  ⊚    stone    mixability with                ⊚                       ◯                              ◯                                   ⊚                                        ⊚                                             ⊚                                                  ⊚    aggregate    mixability with cement                ◯                       ◯                              ◯                                   ◯                                        ◯                                             ◯                                                  ◯                1.0    0.2    0.4  0.9  1.1  1.2  0.1    decompn. time of                ◯                       ◯                              ◯                                   ⊚                                        ⊚                                             ⊚                                                  ⊚    emulsion    ______________________________________

                  TABLE 7    ______________________________________                 Ex.    Additives (pts. by wt.)                   129    130    131  132  133  134    ______________________________________    Component A-1    tallow-dipropylenetriamine             0.2  0.2    tallow-tripropylenetetramine                          0.3    0.2    tallow-    tetrapropylenepentamine    tallow-    pentapropylenehexamine    adduct of tallow-dipropylene-    triamine with EO (n = 15)    adduct of tallow-tripropylene-                   0.2                0.2  0.3    tetramine with EO (n = 10)    adduct of tallow-tripropylene-    tetramine with PO (n = 10)    adduct of tallow-tetrapro-    pylenepentamine with PO    (n = 7)    tallow-alkanoyldiethylene-        0.2    triamine    aminated lignin                   0.2           0.2    stearylimidazoline    0.2    laurylbetanine    Component B    gallnut tannic acid          0.3    quebracho tannic acid                   0.2    0.2         0.2  0.3  0.3    catechol    resorcinol    hydroquinone    pyrogallol     0.1    gallic acid           0.1    methyl gallate    Components C and D    calcium ligninsulfonate                          0.1    0.1       0.2  0.2    sodium gluconate                   0.1                0.1    polyethylene glycol          0.2  0.1  0.1  0.2    (MW = 400)    glycerol       0.2    sorbitol              0.2    Penetration of asphalt    (1/10 mm)    60-80          ◯    80-100                ◯                                      ◯                                           ◯                                                ◯    150-200                      ◯    Results of    examinations    radial compression strength                   4.3    4.3    4.0  3.9  4.1  4.0    (kgf/cm.sup.2)    storage stability of emulsion                   ◯                          ◯                                 ◯                                      ◯                                           ◯                                                ◯                   1.2    2.0    2.2  2.5  1.8  1.7    adherence to crushed stone                   ⊚                          ⊚                                 ⊚                                      ⊚                                           ⊚                                                ⊚    mixability with aggregate                   ⊚                          ⊚                                 ⊚                                      ⊚                                           ⊚                                                ⊚    mixability with cement                   ◯                          ◯                                 ◯                                      ◯                                           ◯                                                ◯                   0.2    0.2    0.3  0.2  0.3  0.2    decompn. time of emulsion                   ⊚                          ⊚                                 ⊚                                      ⊚                                           ⊚                                                ⊚    ______________________________________

                  TABLE 8    ______________________________________              Comp. Ex.    Additives (pts. by wt.)                101    102    103  104  105  106  107    ______________________________________    Component A-1    tallow-     0.5    dipropylenetriamine    tallow-            0.5    tripropylenetetramine    tallow-tetra-             0.5    propylenepentamine    tallow-penta-                  0.5    propylenehexamine    adduct of                           0.6    tallow-dipropylene    triamine with EO    (n = 15)    adduct of                                0.6    tallow-tripropylene-    tetramine with EO    (n = 10)    adduct of                                     0.6    tallow-tripropylene-    tetramine with PO    (n = 10)    adduct of    tallow-tetrapro-    pylenepentanine with    PO (n = 7)    tallow-    alkanoyldiethylene-    triamine    animated lignin    stearylimidazoline    laurylbetanine    Component B    gallnut tannic acid    quebracho tannic acid    catechol    resorcinol    hydroquinone    pyrogallol    gallic acid    methyl gallate    Components C and D    calcium                   0.2    ligninsulfonate    sodium gluconate                         0.1    polyethylene glycol                 0.1    (MW = 400)    glycerol    sorbitol                                 0.1    Penetration of asphalt    (1/10 mm)    60-80       ◯      ◯  ◯    80-100             ◯    ◯    150-200                   ◯  ◯    Results of    examinations    radial compression                1.8    1.7    1.8  1.6  1.9  1.7  1.9    strength (kgf/cm.sup.2)    storage stability of                ◯                       ◯                              ◯                                   X    X    ◯                                                  X    emulsion    2.6    3.4    4.7  6.5  5.2  4.0  5.4    adherence to crushed                Δ                       Δ                              Δ                                   X    X    X    X    stone    mixability with                Δ                       Δ                              Δ                                   Δ                                        Δ                                             Δ                                                  Δ    aggregate    mixability with cement                X      X      X    X    X    X    X                8.5    8.7    3.9  9.1  6.5  4.7  5.8    decompn. time of                Δ                       Δ                              Δ                                   Δ                                        Δ                                             Δ                                                  Δ    emulsion    ______________________________________

                  TABLE 9    ______________________________________              Comp. Ex.    Additives (pts. by wt.)                108    109    110  111  112  113  114    ______________________________________    Component A-1    tallow-    dipropylenetriamine    tallow-    tripropylenetetramine    tallow-tetra-    propylenepentamine    tallow-penta-    propylenehexamine    adduct of    tallow-dipropylene    triamine with EO    (n = 15)    adduct of                                0.2    tallow-tripropylene-    tetramine with EO    (n = 10)    adduct of                                     0.3    tallow-tripropylene-    tetramine with PO    (n = 10)    adduct of   0.6    tallow-tetrapro-    pylenepentanine with    PO (n = 7)    tallow-            0.5    alkanoyldiethylene-    triamine    animated lignin           1.0    stearylimidazoline             0.8            0.2    laurylbetanine                      0.7  0.2    Component B    gallnut tannic acid    quebracho tannic acid    catechol    resorcinol    hydroquinone    pyrogallol    gallic acid    methyl gallate    Components C and D    calcium                                  0.2    ligninsulfonate    sodium gluconate    polyethylene glycol    (MW = 400)    glycerol    0.3                               0.2    sorbitol    Penetration of asphalt    (1/10 mm)    60-80                          ◯  ◯    80-100      ◯                       ◯    ◯    150-200                   ◯  ◯    Results of    examinations    radial compression                1.8    1.7    1.7  1.9  1.7  1.6  1.8    strength (kgf/cm.sup.2)    storage stability of                X      X      ◯                                   ◯                                        ◯                                             ◯                                                  ◯    emulsion    5.3    6.3    4.0  4.2  3.7  3.0  3.1    adherence to crushed                X      Δ                              Δ                                   X    X    X    X    stone    mixability with                Δ                       Δ                              Δ                                   Δ                                        X    Δ                                                  Δ    aggregate    mixability with cement                X      X      X    X    X    X    X                4.6    4.3    4.5  8.1  8.2  3.6  5.0    decompn. time of                Δ                       Δ                              Δ                                   Δ                                        X    X    Δ    emulsion    ______________________________________

                  TABLE 10    ______________________________________                 Comp. Ex.    Additives (pts. by wt.)                   115    116    117  118  119  120    ______________________________________    Component A-1    tallow-dipropylenetriamine    tallow-tripropylenetetramine    tallow-               0.6    tetrapropylenepentamine    tallow-    pentapropylenehexamine    adduct of tallow-dipropylene-                                 0.5    triamine with EO (n = 15)    adduct of tallow-tripropylene-                   0.3                0.6    tetramine with EO (n = 10)    adduct of tallow-tripropylene-    tetramine with PO (n = 10)    adduct of tallow-tetrapro-             0.5    pylenepentamine with PO    (n = 7)    tallow-alkanoyldiethylene-                  0.2    triamine    aminated lignin                   0.2                          0.2    stearylimidazoline    laurylbetanine    Component B    gallnut tannic acid    quebracho tannic acid    catechol    resorcinol    hydroquinone    pyrogallol    gallic acid    methyl gallate    Components C and D    calcium ligninsulfonate                   0.1    sodium gluconate    polyethylene glycol                   0.1    (MW = 400)    glycerol    sorbitol    Penetration of asphalt    (1/10 mm)    60-80                        ◯    80-100         ◯      ◯                                                ◯    150-200               ◯    ◯    Results of    examinations    radial compression strength                   1.7    1.8    1.7  1.8  1.7  1.9    (kgf/cm.sup.2)    storage stability of emulsion                   ◯                          ◯                                 X    ◯                                           X    ◯                   2.9    4.4    5.4  4.8  5.7  4.6    adherence to crushed stone                   X      Δ                                 X    X    X    Δ    mixability with aggregate                   Δ                          Δ                                 Δ                                      Δ                                           Δ                                                Δ    mixability with cement                   X      X      X    X    X    X                   3.7    7.9    7.0  4.1  4.3  3.9    decompn. time of emulsion                   Δ                          Δ                                 Δ                                      Δ                                           Δ                                                Δ    ______________________________________

                  TABLE 11    ______________________________________              Comp. Ex.    Additives (pts. by wt.)                121    122    123  124  125  126  127    ______________________________________    Component A-1    tallow-     0.5    propylenediamine    adduct of tallow-  0.5    propylenediamine with    EO (n = 3)    tallow-monoamine*         0.5    adduct of                      0.5    tallow-monoamine    with PO (n = 7)**    stearyl-                            0.6    trimethylammonium    chloride    polyoxyethylene                          1.0    nonylphenyl ethyl    (n = 85)    sodium                                        0.6    dodecylbenzenesulfate    sodium oleate    Component B    gallnut tannic acid                       0.3    quebracho tannic acid                    0.5    catechol    resorcinol    hydroquinone    pyrogallol                0.3    gallic acid    methyl gallate    Components C and D    calcium                             0.2    ligninsulfonate    sodium gluconate    polyethylene glycol                           0.3    (MW = 400)    glycerol    sorbitol    Penetration of asphalt    (1/10 mm)    60-80       ◯      ◯  ◯    80-100             ◯    ◯    150-200                   ◯  ◯    Results of    examinations    radial compression                1.8    2.8    2.9  1.7  2.0  1.5  1.8    strength (kgf/cm.sup.2)    storage stability of                ◯                       ◯                              X    X    X    ◯                                                  ◯    emulsion    4.5    3.5    5.4  6.5  6.4  3.3  4.5    adherence to crushed                X      ◯                              ◯                                   Δ                                        X    Δ                                                  X    stone    mixability with                X      Δ                              Δ                                   X    X    ⊚                                                  X    aggregate    mixability with cement                X      ◯                              X    ◯                                        ◯                                             ◯                                                  X                9.3    1.4    2.8  1.6  0.3  0.1  3.7    decompn. time of                X      X      X    X    Δ                                             Δ                                                  X    emulsion    ______________________________________     notes)     *it refers a mono(tallowalkyl)amine (the same applies also to the     following Table).     **it refers an adduct of amono(tallowalkyl)amine with propylene oxide (th     same applies also to the following Table).

                  TABLE 12    ______________________________________              Comp. Ex.  Ex.    Additives (pts. by wt.)                128    129    130  135  136  137  139    ______________________________________    Component A-1    tallow-            0.3    propylenediamine    adduct of tallow-              0.2    propylenediamine with    EO (n = 3)    tallow-monoamine   0.3                        0.2    adduct of                      0.4    tallow-monoamine    with PO (n = 7)    stearyl-                            0.4  0.3    trimethylammonium    chloride    polyoxyethylene           1.0                 0.5    nonylphenyl ethyl    (n = 85)    sodium                              0.2       0.2    dodecylbenzenesulfate    sodium oleate                0.6                          0.5    Component B    gallnut tannic acid       0.2    quebracho tannic acid          0.3       0.3  0.2    catechol                  0.2    resorcinol    hydroquinone    pyrogallol                                    0.2    gallic acid                         0.3    methyl gallate                           0.1    Components C and D    calcium                        0.1            0.1    ligninsulfonate    sodium gluconate                    0.1    polyethylene glycol                0.3                0.1       0.2  0.1    (MW = 400)    glycerol    sorbitol                            0.2       0.1    Penetration of asphalt    (1/10 mm)    60-80                          ◯                                             ◯    80-100      ◯ ◯       ◯    150-200            ◯    ◯    Results of    examinations    radial compression                1.7    1.7    2.2  3.0  2.8  3.0  2.7    strength (kgf/cm.sup.2)    storage stability of                X      ◯                              ◯                                   ◯                                        ◯                                             ◯                                                  ◯    emulsion    5.5    3.6    3.2  3.4  4.3  3.2  2.2    adherence to crushed                X      X      Δ                                   ◯                                        ◯                                             ◯                                                  ◯    stone    mixability with                X      X      ◯                                   Δ                                        Δ                                             Δ                                                  ◯    aggregate    mixability with cement                X      X      X    ◯                                        ◯                                             ◯                                                  ◯                9.5    8.6    3.2  1.6  1.8  1.8  1.5    decompn. time of                X      X      Δ                                   Δ                                        Δ                                             Δ                                                  Δ    emulsion    ______________________________________

As shown in Tables 3 to 12, Examples of the present invention aresuperior to Comparative Examples in various performances evaluated.

It will be apparent that the same can be varied in many processes,although the present invention has been thus illustrated. Suchvariations should not be regarded as deviated from the attempt and scopeof the present invention. And it is considered that all of such themodifications apparent to any person skilled in the art are included inthe scope of the following claims.

We claim:
 1. An additive composition for an asphalt emulsion whichcomprises (B) a polyphenolic compound, and at least one member selectedfrom the group consisting of (C) anionic polymeric dispersants,hydroxycarboxylic acids and water-soluble salts of hydroxycarboxylicacids and (D) saccharides, sugar alcohols and polyhydric alcohols. 2.The additive composition for an asphalt emulsion as described in claim1, which further comprises (A) an emulsifier.
 3. The additivecomposition for an asphalt emulsion as described in claim 2, whereincomponent (A) is at least one member selected from the group consistingof aliphatic amines represented by the following formula (1): ##STR6##wherein R¹ is a hydrocarbon group or acyl group having 8 to 22 carbonatoms; R² is a hydrocarbon group having 8 to 22 carbon atoms, a hydrogenatom or a group represented by the formula: (AO)_(m) --H wherein AOrepresents an oxyalkylene group having 2 or 3 carbon atoms; and mrepresents a number of 1 to 30; R³ is a hydrogen atom or a grouprepresented by the formula: (AO)_(m) --H wherein AO and m are those asthe above definitions; R⁴ is a hydrogen atom or a group represented bythe formula: (AO)_(m) --H wherein AO and m are those as the abovedefinitions; A is an ethylene group or a propylene group; and p is aninteger of 2 to 5, aminated lignins, imidazolines having a hydrocarbongroup having 7 or more carbon atoms, betaines having a hydrocarbon grouphaving 7 or more carbon atoms and amidobetaines having a hydrocarbongroup having 7 or more carbon atoms.
 4. The additive composition for anasphalt emulsion as described in claim 1, wherein component (B) is atleast one member selected from the group consisting of tannic acid,tannin compounds, catechol, resorcinol, hydroquinone, pyrogallol, gallicacid and gallic acid derivaties.
 5. The additive composition for anasphalt emulsion as described in claim 1, wherein component (C) is atleast one member selected from the group consisting of ligninsulfonicacid, water-soluble salts of lignin-sulfonic acid and sodium gluconate.6. The additive composition for an asphalt emulsion as described inclaim 1, wherein component (D) is at least one member selected from thegroup consisting of sorbitol, polyethylene glycols having an averagemolecular weight of 200 to 5000, and glycerol.
 7. An asphalt emulsioncomprising asphalt, water, (A) an emulsifier and the additivecomposition for asphalt emulsion as described in claim
 1. 8. The asphaltemulsion as described in claim 7, wherein component (B) is at least onemember selected from the group consisting of tannic acid, tannincompounds, catechol, resorcinol, hydroquinone, pyrogallol, gallic acidand gallic acid derivaties.
 9. The asphalt emulsion as described inclaim 8, wherein component (C) is at least one member selected from thegroup consisting of ligninsulfonic acid, water-soluble salts ofligninsulfonic acid and sodium gluconate.
 10. The asphalt emulsion asdescribed in claim 8, wherein component (D) is at least one memberselected from the group consisting of sorbitol, polyethylene glycolshaving an average molecular weight of 200 to 5000, and glycerol.
 11. Theasphalt emulsion as described in claim 8, wherein component (A) is atleast one member selected from the group consisting of aliphatic aminesrepresented by the following formula (1): ##STR7## wherein R¹ is ahydrocarbon group or acyl group having 8 to 22 carbon atoms; R² is ahydrocarbon group having 8 to 22 carbon atoms, a hydrogen atom or agroup represented by the formula: (AO)_(m) --H wherein AO represents anoxyalkylene group having 2 or 3 carbon atoms; and m represents a numberof 1 to 30; R³ is a hydrogen atom or a group represented by the formula:(AO)_(m) --H wherein AO and m are those as the above definitions; R⁴ isa hydrogen atom or a group represented by the formula: (AO)_(m) --Hwherein AO and m are those as the above definitions; A is an ethylenegroup or a propylene group; and p is an integer of 2 to 5, aminatedlignins, imidazolines having a hydrocarbon group having 7 or more carbonatoms, betaines having a hydrocarbon group having 7 or more carbon atomsand amidobetaines having a hydrocarbon group having 7 or more carbonatoms.
 12. The asphalt emulsion as described in claim 8, whichcomprises, per 100 parts by weight of the total of asphalt and water, 35to 90 parts by weight of asphalt, 65 to 10 parts by weight of water,0.01 to 10 parts by weight of component (B) and 0.01 to 10 parts byweight of at least one member selected from the group consisting ofcomponents (C) and (D).
 13. The asphalt emulsion as described in claim8, which comprises, per 100 parts by weight of the total of asphalt andwater, 35 to 90 parts by weight of asphalt, 65 to 10 parts by weight ofwater, 0.01 to 10 parts by weight of component (A), 0.01 to 10 parts byweight of component (B) and 0.01 to 10 parts by weight of at least onemember selected from the group consisting of components (C) and (D). 14.A paving composition comprising aggregate and the asphalt emulsion asdescribed in claim
 8. 15. A composition for an asphalt emulsion whichcomprises (A-1) at least one member selected from the group consistingof aliphatic amines represented by the following formula (1): ##STR8##wherein R¹ is a hydrocarbon group or acyl group having 8 to 22 carbonatoms; R² is a hydrocarbon group having 8 to 22 carbon atoms, a hydrogenatom or a group represented by the formula: (AO)_(m) --H wherein AOrepresents an oxyalkylene group having 2 or 3 carbon atoms; and mrepresents a number of 1 to 30; R³ is a hydrogen atom or a grouprepresented by the formula: (AO)_(m) --H wherein AO and m are those asthe above definitions; R⁴ is a hydrogen atom or a group represented bythe formula: (AO)_(m) --H wherein AO and m are those as the abovedefinitions; A is an ethylene group or a propylene group; and p is aninteger of 2 to 5, aminated lignins, imidazolines having a hydrocarbongroup having 7 or more carbon atoms, betaines having a hydrocarbon grouphaving 7 or more carbon atoms and amidobetaines having a hydrocarbongroup having 7 or more carbon atoms; and (B) a polyphenolic compound.16. The composition for asphalt emulsion as described in claim 15, whichfurther comprises (C) at least one member selected from the groupconsisting of anionic polymeric dispersants, hydroxycarboxylic acids andwater-soluble salts of hydroxycarboxylic acids, and/or, (D) at least onemember selected from the group consisting of saccharides, sugar alcoholsand polyhydric alcohols.
 17. The composition for asphalt emulsion asdescribed in claim 16, wherein component (C) is at least one memberselected from the group consisting of ligninsulfonic acid, water-solublesalts of lignin-sulfonic acid and sodium gluconate.
 18. The compositionfor asphalt emulsion as described in claim 17, wherein component (D) isat least one member selected from the group consisting of sorbitol,polyethylene glycols having an average molecular weight of 200 to 5000,and glycerol.
 19. The composition for asphalt emulsion as described inclaim 16, wherein component (B) is at least one member selected from thegroup consisting of tannic acid, tannin compounds, catechol, resorcinol,hydroquinone, pyrogallol, gallic acid and gallic acid derivaties.
 20. Anasphalt emulsion comprising asphalt, water and the composition forasphalt emulsion as described in claim
 16. 21. The asphalt emulsion asdescribed in claim 20, which comprises, per 100 parts by weight of thetotal of asphalt and water, 40 to 80 parts by weight of asphalt, 60 to20 parts by weight of water, 0.01 to 10 parts by weight of component (A)and 0.01 to 5 parts by weight of component (B).
 22. The asphalt emulsionas described in claim 21, which further comprises, per 100 parts byweight of the total of asphalt and water, 0.01 to 10 parts by weight of(C) at least one member selected from the group consisting of anionicpolymeric dispersants, hydroxycarboxylic acids and water-soluble saltsof hydroxycarboxylic acids, and 0.01 to 10 parts by weight of (D) atleast one member selected from the group consisting of saccharides,sugar alcohols and polyhydric alcohols.
 23. A paving compositioncomprising aggregate and the asphalt emulsion as described in claim 20,wherein the amount of the aggregate is 75 to 95 parts by weight and theamount of the asphalt emulsion is 25 to 5 parts by weight per 100 partsby weight of the total of the aggregate and the asphalt emulsion.
 24. Acomposition for emulsification which comprises water, (A) an emulsifier,(B) a polyphenolic compound, and (C) at least one member selected fromthe group consisting of anionic polymeric dispersants, hydroxycarboxylicacids and water-soluble salts of hydroxycarboxylic acids, and/or, (D) atleast one member selected from the group consisting of saccharides,sugar alcohols and polyhydric alcohols.
 25. The composition foremulsification as described in claim 24, which contains component (C)and component (D).
 26. The composition for emulsification as describedin claim 25, which further comprises a monobasic acid.
 27. A process forthe preparation of the composition for emulsification as described inclaim 25, which comprises step 1 of adding a mixture of component (A)and component (D) to an aqueous solution of component (B) to prepare anaqueous solution and step 2 of adding an aqueous solution of component(C) to the obtained aqueous solution.
 28. The composition foremulsification as described in claim 24, which further comprises amonobasic acid.
 29. A process for the preparation of the composition foremulsification as described in claim 26, which comprises step 1 ofadding a monobasic acid to an aqueous solution of component (B) toprepare an aqueous acidic solution, step 2 of adding a mixture ofcomponent (A) and component (D) to the aqueous acidic solution toprepare an aqueous solution, and step 3 of adding an aqueous solution ofcomponent (C) to the obtained aqueous solution.
 30. A composition foremulsification which comprises water, (A-1) at least one member selectedfrom the group consisting of aliphatic amines represented by thefollowing formula: ##STR9## wherein R¹ is a hydrocarbon group or acylgroup having 8 to 22 carbon atoms; R² is a hydrocarbon group having 8 to22 carbon atoms, a hydrogen atom or a group represented by the formula:(AO)_(m) --H wherein AO represents an oxyalkylene group having 2 or 3carbon atoms; and m represents a number of 1 to 30; R³ is a hydrogenatom or a group represented by the formula: (AO)_(m) --H wherein AO andm are those as the above definitions; R⁴ is a hydrogen atom or a grouprepresented by the formula: (AO)_(m) --H wherein AO and m are those asthe above definitions; A is an ethylene group or a propylene group; andp is an integer of 2 to 5, aminated lignins, imidazolines having ahydrocarbon group having 7 or more carbon atoms, betaines having ahydrocarbon group having 7 or more carbon atoms and amidobetaines havinga hydrocarbon group having 7 or more carbon atoms; and (B) apolyphenolic compound.
 31. The composition for emulsification asdescribed in claim 30, which further comprises (C) at least one memberselected from the group consisting of anionic polymeric dispersants,hydroxycarboxylic acids and water-soluble salts of hydroxycarboxylicacids and (D) at least one member selected from the group consisting ofsaccharides, sugar alcohols and polyhydric alcohols.
 32. The compositionfor emulsification as described in claim 31, which further comprises amonobasic acid.
 33. A process for the preparation of the composition foremulsification as described in claim 32, which comprises step 1 ofadding a monobasic acid to an aqueous solution of component (B) toprepare an aqueous acidic solution, step 2 of adding a mixture ofcomponent (A-1) and component (D) to the aqueous acidic solution toprepare an aqueous solution, and step 3 of adding an aqueous solution ofcomponent (C) to the obtained aqueous solution.
 34. A process for thepreparation of the composition for emulsification as described in claim31, which comprises step 1 of adding a mixture of component (A-1) andcomponent (D) to an aqueous solution of component (B) to prepare anaqueous solution, and step 2 of adding an aqueous solution of component(C) to the obtained aqueous solution.
 35. The composition foremulsification as described in claim 30, which further comprises amonobasic acid.
 36. The composition for emulsification as described inclaim 30, which further comprises a water-soluble inorganic salt.
 37. Aprocess for emulsifying asphalt in water, which comprises adding moltenasphalt to the composition for emulsification as described in claim 24or 32 to prepare a mixture, and then emulsifying the mixture.